SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Hesong Wang,Jinlong Wang,Jing Zhao,Han Zhang,Luming Liu,Xueying Sun,Guibai Li,Heng Liang
As an emerging metal organic framework (MOF) material, MIL-101(Cr) has a large specific surface area and good hydraulic stability, making it ideal in applications before ultrafiltration (UF). However, the unclear interaction between MIL-101(Cr) and natural organic matter (NOM) was identified as the main limitation to understand membrane fouling. To reveal the working mechanisms of NOM removal using MIL-101(Cr), an integrated system of MOF and UF was constructed and operated in separation mode (SM) and coating mode (CM). Based on the results, MIL-101(Cr) had a high NOM adsorption capacity of 68.454 mg/g for HA and 174.725 mg/g for BSA at saturation. Permeate quality improvement occurred in both modes over a 37.7% UV 254 removal rate and a 15% fluorescence intensity decrease, and permeation performance of the hybrid system was simultaneously enhanced. We found that MIL-101(Cr) influenced membrane fouling behaviors and models because of the foulant transformation in SM and dispersed NOM in the MIL-101(Cr) layer in CM. Furthermore, MIL-101(Cr) played a dual role in the integrated system. It could remove NOM by adsorption, leading to membrane fouling reduction, but also caused additional filtration resistance. Notably, MIL-101(Cr) showed the overall positive effects due to its open hollow structure and good hydrophilicity. The π-π interactions and salt-bridges between MIL-101(Cr) and NOM played a dominant role in adsorption. Whilst SM was more efficient in membrane fouling mitigation due to reduced membrane fouling resistance and a normalized flux increase above 15%, CM could achieve the same permeate quality with less MIL-101(Cr) usage and reaction time. This study reveals the interaction between MIL-101(Cr) and NOM and their effects on UF, providing a scientific basis for the widespread application of MOFs.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Dongmei Jia,Yuejin Li,Huamin Cai,Yongzheng Duan,Jing Li,Chen Ling
Capture of heavy metal ions from aqueous solutions is a critical but challenging step in environmental treatment. In this work, NH2-MIL-101(Fe) nanoparticles were synthesized by simple solvothermal methods and applied to capture Cr(VI) anions from aqueous solutions. The results revealed that NH2-MIL-101(Fe) exhibited a high capture capacity (375.2 mg g–1) and an ultrafast capture rate (4 min reaching equilibrium). The competitive effects of coexisting ions such as Cl–, HCO3–, PO43–, Cd2+, Ca2+, and Cu2+ on Cr(VI) are very weak, suggesting that the adsorption selectivity significantly enhanced by loading amino groups on MIL-101(Fe). Density functional theory (DFT) calculation was performed to better understand the adsorption mechanism of Cr(VI), showing that the amino groups could increase the adsorption energy of Cr(VI) for enhancing the adsorption capacity. Based on powder X-ray diffraction, X-ray photoelectron spectroscopy, and DFT calculations, the Cr(VI) capture mechanism by NH2-MIL-101(Fe) nanoparticles was a combination of coordination between Fe and Cr(VI), electrostatic interaction between Cr2O72– and the protonated amino group, and reduction of Cr(VI) to Cr(III).
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Jun Liu,Hui Wang,Wen-Yao Zhu,Heng-Xue Xie,Xin Li,Wen-Juan Li,Ge Bai,Meng-Jie Chang,Xiao-Jiao Chai,Hui-Ling Du,Shi-Jie Song
We present a novel method to facilely prepare magnetically recoverable AgCl/Fe 3 O 4 @MIL-100(Fe) (ACFM) nanostructures for photocatalytic degradation of rhodamine B (RhB). The ACFM was directly prepared via a simple successive ionic layer adsorption and reaction (SILAR) deposition of MIL-100(Fe) on solvothermal synthesized Ag/Fe 3 O 4 nanoparticles , in which process Ag was completely oxidized into AgCl concurrent with the formation of MIL-100(Fe). The ACFM prepared with 15 SILAR cycles exhibits 92.9% efficiency towards photodegrading RhB within 30 min under visible light illumination, which is higher than that of the individual structure of AgCl/Fe 3 O 4 , Ag/Fe 3 O 4 @MIL-100(Fe) or Fe 3 O 4 @MIL-100(Fe). The remarkably enhanced photocatalytic performance is attributed to the abundant active sites and sufficient visible light response of MIL-100(Fe), as well as effective charge separation at the heterojunction interface between AgCl and MIL-100(Fe). Furthermore, the obtained ACFM can be quickly separated from the pollutant solution with a magnet and possesses good stability for recycling photocatalysis . In light of the study, the ACFM nanostructures are believed to be applied as promising photocatalysts for practical applications.
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JOURNAL OF CLUSTER SCIENCE
·
2023
·Vol. 34
·期 6
·3095-3103
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IF 2.8
Liu Xiangyi,Zheng Qianye,Jia Deqi,Wang Wenwen,Zhao Hong,Tao Xiansen,Sha Jingquan
To explore novel nanozymes as colorimetric biosensors with highly activities, the ternary MIL-101(Fe)@P 2 W 18 @SWNT nanocomposite was successfully fabricated based on the optimal matching principle, namely, Wells–Dawson-type polyoxometalates (POMs, H 6 P 2 W 18 O 62 abbreviated as P 2 W 18 ) were encapsulated in a custom MIL-101(Fe) cavity, and single-walled carbon nanotubes (SWNT) was then fixed. The peroxidase-like activities of MIL-101(Fe)@P 2 W 18 @SWNT nanocomposite were evaluated by detecting hydrogen peroxide (H 2 O 2 ) and glucose (GLC). Compared with the MIL-101(Fe), P 2 W 18 and SWNT, the MIL-101(Fe)@P 2 W 18 @SWNT exhibits better peroxidase-like properties and stability due to the nature of all components and their optimal synergy. Based on the excellent catalytic activity of MIL-101(Fe)@P 2 W 18 @SWNT , two colorimetric biosensors for detecting H 2 O 2 and GLC with linear ranges of 0–80 μM (H 2 O 2 ) and 0–150 μM (GLC) were constructed, and the low detection limit of 0.3 μM for H 2 O 2 and 0.2 μM for GLC are superior to the most reported nanozymes. The work opens a promising route in constructing heterogeneous MOFs and POMs-based nanozymes for biosensing application.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 14
·40534-40550
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IF 5.8
Fang Lei,Wu Guojian,Yao Keyu,Zhang Dongyang,Zhou Yongchao
A novel heterogeneous catalyst named MoS 2 /MIL-53(Fe, Cu) (MMFC) was prepared by hydrothermal method and applied in a heterogeneous electro-Fenton (hetero-EF) system for lomefloxacin (LOM) degradation in this work. Under the optimal conditions of current density 3 mA/cm 2 , catalyst dosage 0.100 g/L, and initial pH 6, 93.5% LOM (2 mg/L) removal efficiency was achieved in the MMFC hetero-EF system within 60 min, indicating an obvious improvement compared with the MIL-53(Fe, Cu) hetero-EF system. The good catalytic activity was attributed to more effective active sites of the catalyst and the conversion of Fe(II)/Fe(III) and Cu(I)/Cu(II) promoted by Mo(IV) in MoS 2 , which could be inferred by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) characterizations. The reusability and stability of MMFC were explored based on five cyclic experiments, and the average degradation efficiency reached 73.9%. Furthermore, the hetero-EF system could achieve the total removal of moxifloxacin and tetracycline within 6 min and 40 min, respectively. Quenching experiments revealed that the hydroxyl radicals (·OH) were the main reactive radicals while superoxide radicals (·O 2 − ) and singlet oxygen ( 1 O 2 ) played a certain part in LOM degradation. Finally, the possible mechanism of the hetero-EF process and LOM degradation pathways were proposed, including substitution, elimination, and cleavage of ring structures. Accounting for good catalytic performance, low preparation cost, and satisfactory versatility, the MMFC exhibited good potential to work as a hetero-EF catalyst for wastewater treatment.
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OPTICAL MATERIALS
·
2022
·
IF 3.754
Hao Hu,Jiacheng Jin,Mingchen Xu,Chengdong Xu,Yue Cheng,Weiwei Ji,Zhencen Ding,Min Shao,Yushan Wan
The present work demonstrates the synthesis of the microsphere composite photocatalyst Bi 3 O 4 Br/NH 2 -MIL-125(Ti) (BOB/NMILT) system, and the physicochemical properties of the material were analyzed by various characterization means. Further, the photocatalytic performance of the BOB/NMILT system was evaluated by degrading tetracycline (TC) under simulated sunlight. The degradation rate of TC using BOB/NMILT-5 reached 88.5% within 90 min. The degradation rate is 6.5 times and 3 times higher than that of individual catalysts NH 2 -MIL-125(Ti) (NMILT) and Bi 3 O 4 Br, respectively. The improvement in photocatalytic activity of composites mainly benefited from the construction of heterojunctions , which effectively inhibited the recombination of carriers. Importantly, the role of h + and •O 2 − was found to be significant in the reaction of TC. Cumulatively, a Z-scheme photocatalytic degradation mechanism of tetracycline on the BOB/NMILT composite system was proposed. The proposal of this system is of great significance for the future development of photocatalytic materials that can degrade tetracycline.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Meng Zhang,Yu Zhang,Yucong Chen,Xiaoru Tian,Lingzhi Liu,Yizhong Wang,Ruijie Guo,Hong Yan
MIL-88(Fe) was used as an oxidant and a hard template for the synthesis of polypyrrole (PPy) on its surface, and the formation of PPy made the surface of MIL-88(Fe) rougher as well as more voids formed in the interior. The increased specific surface area allowed more benzotriazole (BTA) (17.8 wt%) loaded on PPy/MIL-88 particles. BTA/PPy/MIL-88(Fe) was employed as a novel corrosion inhibitor to enhance the corrosion resistance of epoxy coating for carbon steel. BTA/PPy/MIL-88(Fe) filler improved the corrosion resistance of EP coating without/with artificial scratch by delaying the cathodic and anodic reactions in corrosive media. Both BTA and MIL-88(Fe) played the role of corrosion inhibitors, making EP coating possess active corrosion protection and pH-sensitive performance. Besides, BTA/PPy/MIL-88(Fe) enhanced the adhesion of EP coating by filling the pores inside.
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Molecular Catalysis
·
2022
·
IF 5.089
Weiwen Wang,Jianing Qu,Chaojie Li,Lexin Guo,Xianxin Fang,Guanghui Chen,Jihai Duan
Biomimetic photocatalytic nitrogen fixation is considered as a potential alternative to the Haber-Bosch method, which is an ideal pathway for nitrogen reduction. The development of efficient bionanocatalysts is a serious challenge in the current field of biomimetic nitrogen fixation. Here, we introduced a second metal in the MIL-88A/Fe mesh by metal doping to build a Mo-doped MIL-88A(Fe/Mo)/Fe mesh biomimetic system. The catalyst is a rod-like structure synthesized in situ by hydrothermal method using iron mesh as the substrate, and its rough surface is favorable for the adsorption of N 2 . The introduction of Mo provides a two-electron transfer pathway for the reaction, and the formation of the "MoFe cofactor" effectively promotes charge separation and inhibits the photoelectron-hole complexation. In addition, we kept the catalyst above the liquid surface and provided the proton source through water vapor, which solved the problem of the low solubility of N 2 in water and poor mass transfer efficiency. The results show that the biomimetic photocatalyst has good photoresponsiveness in the whole visible region, and the synergistic effect between the two metals makes the MIL-88A (Fe/Mo 0.017 )/Fe mesh exhibit better photocatalytic performance, and its nitrogen fixation efficiency reaches about 9.6 times that of the original MIL-88A/Fe mesh. This study provides a new idea for the design of photocatalytic ammonia biomimetic photocatalysts.
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DESALINATION
·
2022
·
IF 11.211
Xiangyunxiu Meng,Ruiwen Luo,Guijie Guo,Yulin Li,Hui Fang,Peng Bai,Jiafei Lyu,Xianghai Guo
Adsorption has been expected to be promising for boron-containing water treatment , boron resources recovery and boron isotopic separation. Although metal-organic frameworks have been demonstrated to be potential adsorbent candidates, in-depth investigation of the structure-performance relationship remains insufficient. Herein, the performance and mechanism of boron adsorption and isotopic separation were systematically investigated with isostructural MOFs. Six isomorphic MIL-100(M) materials with metal species from the third main group (Al, Ga and In) and the fourth period (Sc, Cr and Fe) were solvothermally synthesized as boron adsorbents. Superior boron isotopic separation factors ( S ) with 10 B preference and comparable boron adsorption capacity ( Q ) were observed through batch boron adsorption experiments, where MIL-100(Al) exhibited the highest S of 1.618 and MIL-100(Sc) achieved the largest Q of 8.74 g-B/mol-MOF. A high correlation between metal atomic radius and performance was revealed and a plausible mechanism was proposed for boron adsorption and isotopic separation involving the important role of the metal center through post-adsorption characterization. This study will pave the way for designing boron adsorbents with improved properties and promote the efficient utilization of boron resources in water.
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Materials
·
2022
·Vol. 15
·期 10
·3645
·
IF 3.748
Minmin Zou,Ming Dong,Mingliang Luo,Hexin Zhu,Tian Zhao
Hierarchically porous MIL-101(Cr) (H-MIL-101(Cr)) with meso/macro-pores was directly prepared via nanofusion progress by using butyric acid as a modulating agent. In the methyl orange (MO) adsorption experiments, H-MIL-101(Cr) showed a high adsorption capability of 369.8 mg g−1, which was 1.52-fold greater than that of pristine MIL-101(Cr) (P-MIL-101(Cr)). While in the oxidation reaction of indene and 1-dodecene tests, H-MIL-101(Cr) presented much higher catalytic efficiency, with turnover frequency (TOF) values of 0.7242 mmol g−1min−1and 0.1492 mmol g−1min−1, respectively, which were 28% and 34% greater than that in the case of P-MIL-101(Cr). Thus, compared with P-MIL-101(Cr), H-MIL-101(Cr) exhibited better removal efficiency and higher levels of activity in the oxidation reactions of indene and 1-dodecene. The unique structure of H-MIL-101(Cr) also contributed to its superior performance in these processes.Keywords:hierarchically porous;MIL-101(Cr);butyric acid;MO adsorption;catalysis
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Nanomaterials
·
2022
·Vol. 12
·期 5
·811
·
IF 5.719
Kang-Ping Cui,Yu-Ying He,Kai-Jie Xu,Yu Zhang,Chang-Bin Chen,Zheng-Jiang Xu,Xing Chen
In this work, the combination of high surface area diatomite with Fe and Cu bimetallic MOF material catalysts (Fe0.25Cu0.75(BDC)@DE) were synthesized by traditional solvothermal method, and exhibited efficient degradation performance to tetracycline hydrochloride (TC). The degradation results showed: Within 120 min, about 93% of TC was degraded under the optimal conditions. From the physical–chemical characterization, it can be seen that Fe and Cu play crucial roles in the reduction of Fe3+because of their synergistic effect. The synergistic effect can not only increase the generation of hydroxyl radicals (•OH), but also improve the degradation efficiency of TC. The Lewis acid property of Cu achieved the pH range of reaction system has been expanded, and it made the material degrade well under both neutral and acidic conditions. Loading into diatomite can reduce agglomeration and metal ion leaching, thus the novel catalysts exhibited low metal ion leaching. This catalyst has good structural stability, and less loss of performance after five reaction cycles, and the degradation efficiency of the material still reached 81.8%. High performance liquid chromatography–mass spectrometry was used to analyze the degradation intermediates of TC, it provided a deep insight of the mechanism and degradation pathway of TC by bimetallic MOFs. This allows us to gain a deeper understanding of the catalytic mechanism and degradation pathway of TC degradation by bimetallic MOFS catalysts. This work has not only achieved important progress in developing high-performance catalysts for TC degradation, but has also provided useful information for the development of MOF-based catalysts for rapid environmental remediation.Keywords:Fenton-like catalyst;bimetallic MOF;diatomite;synergistic effect;antibiotics
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CHEMOSPHERE
·
2022
·
IF 8.943
Zhenxiang Yang,Jinhui Zhang,Jun Wang,Yun Hu
The coordination of H 2 O with the metal nodes of MOFs destroys the framework of MOFs, which severely inhibits the application of MOFs in the actual environment. In this work, sandwich-like MIL-101@TiO 2 @PDVB composite was synthesized by in-situ hydrothermal and thermal deposition methods and used for the photocatalytic oxidation of toluene under high humidity. The result showed that the composite material had outstanding hydrophobic property with a water contact angle of 142.5°. When relative humidity (RH) was 60%, MIL-101@TiO 2 @PDVB and MIL-101@TiO 2 exhibited an excellent photocatalytic activity for toluene degradation. When RH was 90%, the photocatalytic activity of MIL-101@TiO 2 was severely inhibited, while MIL-101@TiO 2 @PDVB showed high resistance to water. The semi-encapsulated form of PDVB effectively resisted the erosion of H 2 O while providing enough ·OH, and ensured the effective contact between the composites and toluene molecules. MIL-101@TiO 2 @PDVB also exhibited remarkable adsorption-photocatalytic performance in the degradation of liquid phase organic pollutant. MIL-101@TiO 2 @PDVB maintained high stability in long-term alkali resistance experiment and cyclic reaction test. This work provided new insights for the preparation of hydrophobic MOFs based functional materials and their applications for photocatalytic purification of VOCs.
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